A kind of method for using micro- reaction system inhale heat release coupled reaction
Technical field
The present invention relates to a kind of method for inhaling heat release coupled reaction.
Background technology
In chemical process, have substantial amounts of exothermic reaction and the endothermic reaction and exist, reaction liberated heat is not if
Can make full use of can cause the waste of the energy.Therefore, a kind of reaction that heat release and the endothermic reaction can be integrated is developed
Device causes more and more extensive concern.
Microreactor is micro passage reaction, be using precision processing technology manufacture characteristic size in 10-3000 microns
Between microreactor.The passage of micro-expression process fluid in microreactor is in micron level without referring to that micro- reaction is set
Standby appearance and size size or the size of product, millions of minitype channel can be included inside it.Microreactor
Reaction medium can be gas, liquid or dispersion, carried out for reactant in micro- reaction channel physical reactions or
Chemical reaction.Microreactor is a kind of channel-type reactor continuously flowed in essence, has specific surface area big, transmits speed
Rate is high, and time of contact is short, and accessory substance is few;Without enlarge-effect;It can be continuously produced;Amount of heat can be removed in time, it is safe
The features such as.
Therefore, the suction exothermic reaction in industrial production is carried out in microreactor simultaneously, increase is inhaled between exothermic reaction
Heat exchanger effectiveness, while energy consumption is reduced, the diminution of consersion unit size can be achieved, improve the transformation efficiency of reactant,
Being uniformly distributed for reaction interval temperature is realized simultaneously, focus appearance is not had, ensure that device within the whole production cycle
Even running.
The content of the invention
It is an object of the invention to provide a kind of method for inhaling heat release coupled reaction, this method is simultaneously that heat absorption and heat release is anti-
It should be integrated in a microreactor and carry out, can realize and inhale heat release coupled reaction, improve the heat exchange inhaled between exothermic reaction
Efficiency, reduce energy consumption.
The purpose of the present invention is implemented by following technical scheme, but the present invention can come in fact in different forms
Apply, and should not be construed as being limited to embodiment described in this paper.Conversely, there is provided these embodiments, to cause this
Invention is thorough and complete to those skilled in the art, and will fully pass on the scope of the present invention.
Unless otherwise defined, otherwise all technologies used herein and scientific terminology have such as the technical field of the invention
The identical meanings that are generally understood that of those of ordinary skill.Term used in description herein is to be used to describe specifically
Embodiment, rather than be limited.As the singulative used in this specification and the appended claims
" one ", "one", " described " etc. also include plural form, unless context is clearly indicated otherwise.
The invention provides a kind of method for using micro- reaction system inhale heat release coupled reaction, it is characterised in that:
(1)1# reaction raw materials after purification and 2# reaction raw materials are mixed in 1# reactants mixing apparatus and 2# reactants respectively and set
It is well mixed in standby;
(2)1# reactants and 2# reactants are incorporated into micro-reactor apparatus and carry out inhaling heat release coupled reaction;
(3)Reacted product is introduced between in 1# collection of products equipment and 2# collection of products equipment and collected;
It is the endothermic reaction that what the 1# reactants were carried out, which be exothermic reaction, and 2# reactants are carried out, or 1# reactants carry out be
What the endothermic reaction and 2# reactants were carried out is exothermic reaction;
The micro-reactor apparatus is in series by least two microreactor, and is controlled and coupled by temperature automatic adjustment equipment
Reaction temperature;The microreactor is successively by upper heat-insulation layer, upper zone of heating, at least one micro- conversion zone, lower zone of heating, lower insulation
Layer is formed by stacking;Micro- conversion zone is by upper sealing panel, lower sealing plate and is clipped at least one micro- between two layers of sealing plate
Reaction plate forms;
The micro-reaction plate is provided with the micro- reaction channels of 1# for 1# reactant reactions and the micro- reactions of 2# for 2# reactant reactions
Passage;The micro- reaction channel of the 1# and the micro- reaction channels of 2# are respectively with multiple continuous mixing reaction chambers, and described two micro- reactions
It is in be mutually twisted state between the mixing reaction chamber of passage;
Micro- reaction channel and hybrid reaction cavity wall scribble the catalyst of respective reaction.
Preferably, the exothermic reaction is methanation reaction, partial oxidation reaction of methane, methanol to olefins reaction, Fischer-Tropsch
Synthesis, isomerization reaction, methane catalytic combustion reaction, ammonia catalytic oxidation, sulphur dioxide oxidation, acid-base neutralization are anti-
A kind of reaction in answering;The endothermic reaction is that methane reforming with carbon dioxide, methane-steam reforming, catalysis are split
A kind of reaction in solution, inverse water gas reaction.
Preferably, residence time of the reactant in micro- reaction channel is 0.01-2s, reaction pressure 0.1-
6MPa。
Preferably, the inside diameter ranges of the micro- reaction channels of the 1# and the micro- reaction channels of 2# are 0.1-10mm, and the mixing is anti-
The internal diameter width for answering chamber is 0.2-4 times of micro- reaction channel.
Preferably, the mixing reaction chamber t shape or mushroom shaped.
Preferably, the mixing reaction chamber is L-shaped.
Preferably, there is Y shape baffle plate on the relative micro- reaction channel wall of the mixing reaction chamber.
Preferably, the tangible baffle plates of L on micro- reaction channel wall relative with mixing reaction chamber.
Preferably, there be a baffle plate at the top of the mixing reaction chamber, and on the baffle plate and micro- reaction channel wall
Baffle plate have gap.
Preferably, the micro- reaction channels of the 1# and the micro- reaction channels of 2# between its multiple mixing reaction chamber by being mutually twisted
Overall tortuous or spiral shape afterwards.
Compared with prior art, two kinds of reaction channels are provided with the micro-reaction plate provided in the present invention, and two kinds micro- anti-
Passage is answered with multiple continuous mixing reaction chambers, to be advantageous to being sufficiently mixed for reactant respectively.Further, two kinds of micro- reaction channels
Mixing reaction chamber between in being mutually twisted state, this is effectively increased the heat exchange area inhaled between exothermic reaction, improves
Heat exchange efficiency, reduces energy consumption, while realizes being uniformly distributed for reaction interval temperature, does not have focus appearance, ensure that
Even running of the device within the whole production cycle.On the other hand, micro-reactor apparatus of the invention is inhaling heat release coupled reaction dress
Put it is middle independent assortment is needed according to production, it is simple and convenient, be advantageously implemented the peak use rate of equipment, without obvious enlarge-effect,
The process time of device is shortened, reduce further the production cost of reaction unit.
Other features and advantages of the present invention will be described in detail in subsequent specific embodiment part.
Brief description of the drawings
Accompanying drawing is to be further understood for providing to what is invented, and a part for constitution instruction, with following tool
Body embodiment is used for the present invention at that time, but not rear path between fields limitation of the present invention together.In the accompanying drawings:
Fig. 1 is to inhale a kind of structural representation of embodiment of heat release coupled reaction device;
Fig. 2 is a kind of structural representation of embodiment of micro-reactor apparatus;
Fig. 3 is a kind of structural representation of embodiment of micro-reaction plate(T-shaped mixing reaction chamber);
Fig. 4 is a kind of structural representation of embodiment of micro-reaction plate(Mushroom-shaped mixing reaction chamber);
Fig. 5 is a kind of structural representation of embodiment of micro-reaction plate(L mixing reaction chambers);
Fig. 6 is the structural representation of micro-reactor apparatus another kind embodiment;
Fig. 7 is the structural representation of another embodiment of micro-reaction plate(T-shaped mixing reaction chamber);
Fig. 8 is the structural representation of another embodiment of micro-reaction plate(Mushroom-shaped mixing reaction chamber);
Fig. 9 is the structural representation of another embodiment of micro-reaction plate(L mixing reaction chambers);
Figure 10 is a kind of structural representation of embodiment of micro- reaction channel with T-shaped mixing reaction chamber;
Figure 11 is a kind of structural representation of embodiment of micro- reaction channel with mushroom-shaped mixing reaction chamber;
Figure 12 is a kind of structural representation of embodiment of micro- reaction channel with L-shaped mixing reaction chamber.
Description of reference numerals
The 1# product exit through holes of 10 microreactor, 11 1# reactant entrances through hole 12
The micro- reaction channels of 1# of 13 1# reactant entrances, 14 1# product exits 15
The 2# reactant entrances of 21 2# reactant entrances through hole, 22 2# product exits through hole 23
The micro- baffle plates of 30 mixing reaction chamber of reaction channel 31 of the 2# of 24 2# product exits 25
The 2# reactant mixing apparatus of 32 mixing reaction chamber top flap, 41 1# reactants mixing apparatus 42
The pressure control equipment of 43 1# collection of products equipment, 44 2# collection of products equipment 51
The micro-reactor apparatus of 52 flow-control equipment, 53 temperature automatic adjustment equipment 54.
Embodiment
To make the object, technical solutions and advantages of the present invention clearer, below in conjunction with the specific embodiment of the invention and
Corresponding accompanying drawing is clearly fully described by technical solution of the present invention.Embodiment described herein be merely to illustrate and
The present invention is explained, is not intended to limit the invention, protection scope of the present invention is still defined by claims disclosure of that.
Based on the embodiment in the present invention, what those skilled in the art were obtained under the premise of creative work is not made
Every other embodiment, belongs to the scope of protection of the invention.
Fig. 1 show an example for inhaling heat release coupled reaction apparatus structure schematic diagram, and the device is mixed by 1# reactants
Equipment, 2# reactants mixing apparatus, pressure control equipment, temperature automatic adjustment equipment, flow-control equipment, 1# collection of products are set
Standby, 2# collection of products equipment and it is made up of at least two microreactor, the reactant of one of micro-reactor apparatus goes out
Mouth connects with the reaction-ure inlet of another micro-reactor apparatus by the way that pipeline is corresponding.
The micro-reactor apparatus upper heat-insulation layer, upper zone of heating, upper sealing panel, micro-reaction plate, lower sealing plate, lower heating successively
Layer, lower heat-insulation layer are formed by stacking.Upper heat-insulation layer, upper zone of heating, upper sealing panel are provided with 1# reactant entrances through hole and 2# reacts
Thing entrance through hole, and with 1# reactant entrances on micro-reaction plate and 2# reactant entrances are corresponding communicates;Lower sealing plate, lower heating
Layer, lower heat-insulation layer are provided with 1# product exits through hole and 2# product exit through holes, and with the 1# product exits and 2# on micro-reaction plate
Product exit correspondingly communicates.
Between 1# reactant entrances and 1# product exits on micro-reaction plate and 2# reactant entrances and 2# product exits
Between be respectively equipped with for 1# reactant reactions the micro- reaction channels of 1# and for 2# reactant reactions the micro- reaction channels of 2#, shown 1#
Multiple continuous mixing reaction chambers are carried on micro- micro- reaction channel of reaction channel and 2#, and into mutual between the mixing reaction chamber
Interlocking pattern.
Fig. 2 show an example of above-mentioned micro-reactor apparatus structural representation, wherein the micro- reactions of 1# are logical in this example
Road and the micro- reaction channels of 2# are overall tortuous by being mutually twisted between mixing reaction chamber(Shown in Fig. 3, Fig. 4, Fig. 5).
Fig. 6 show an example of above-mentioned micro-reactor apparatus structural representation, wherein the micro- reactions of 1# are logical in this example
Road and the micro- reaction channels of 2# between mixing reaction chamber by being mutually twisted entirety twist(Shown in Fig. 7, Fig. 8, Fig. 9).
In the above-described example, shown mixing reaction chamber can be T shape(Shown in Figure 10), mushroom shaped can be made(Figure 11
It is shown)Or L shape(Shown in Figure 12), and the mixing reaction chamber on the micro- reaction channels of 1# and the micro- reaction channels of 2# is in phase
Mutual interlocking pattern.
Preferably, there is Y shape baffle plate on the relative micro- reaction channel wall of mixing reaction chamber, and the angle α on Y shape baffle plate
Scope is 0 ° -180 °.In addition, also have a baffle plate at the top of mixing reaction chamber, and the baffle plate and micro- reaction channel wall
On baffle plate have gap.
Preferably, the tangible baffle plates of L on micro- reaction channel wall relative with mixing reaction chamber, and the angle β on L-shaped baffle plate
Scope is 90 ° -180 °.
In above-mentioned suction heat release coupled reaction device application process, controlled by pressure control equipment in each reaction channel
Reaction pressure, the heating-up temperature of micro-reactor apparatus zone of heating is controlled by temperature automatic adjustment equipment, is controlled by flow
Equipment controls to adjust residence time of the reaction raw materials in microreactor.
Wherein, after 1# reaction raw materials are sufficiently mixed in 1# reactant mixing apparatus, micro-reactor apparatus is passed sequentially through
In upper heat-insulation layer, upper zone of heating, the 1# reactant entrance through holes on upper sealing panel enter in micro-reaction plate to be loaded with 1# anti-
With the answering thing catalyst micro- reaction channels of 1#, then 10-1000ms is stopped in micro- reaction channel and mixing reaction chamber and has been carried out sufficiently
After reaction, it introduces 1# collection of products by the 1# product exits through hole export on lower heat-insulation layer, lower zone of heating, lower sealing plate and sets
In standby, 1# products are obtained.At the same time, after 2# reaction raw materials are sufficiently mixed in 2# reactant mixing apparatus, lead to successively
Heat-insulation layer, upper zone of heating, the 2# reactant entrance through holes on upper sealing panel is crossed in micro-reactor apparatus to enter in micro-reaction plate
With the being loaded with 2# reactant catalyst micro- reaction channels of 2#, then 10-1000ms is stopped in micro- reaction channel and mixing reaction chamber
After having carried out sufficient reaction, it is incorporated into by the 1# product exits through hole export on lower heat-insulation layer, lower zone of heating, lower sealing plate
In 2# collection of products equipment, 2# products are obtained.
Preferably, carried out in the micro- reaction channels of the 1# be carried out in the endothermic reaction and the micro- reaction channels of the 2# be
Carried out in exothermic reaction, or the micro- reaction channels of the 1# be carried out in exothermic reaction and the micro- reaction channels of the 2# be heat absorption
Reaction.
Preferably, the exothermic reaction is methanation reaction, partial oxidation reaction of methane, methanol to olefins reaction, Fischer-Tropsch
One kind in synthesis, isomerization reaction, methane catalytic combustion reaction, ammonia catalytic oxidation, sulphur dioxide oxidation is anti-
Should;The endothermic reaction is methane reforming with carbon dioxide, methane-steam reforming, catalytic pyrolysis, coal gas is anti-against the current
A kind of reaction in answering.
Embodiment 1
With CH4And O2Partial oxidation reaction of methane is carried out for 1# reaction raw materials, the reaction is strong exothermal reaction, wherein CH4With O2It
Between ratio be 2:1;With CH4And CO2Methane reforming with carbon dioxide is carried out for 2# reaction raw materials, the reaction is the endothermic reaction,
Wherein CH4With CO2Between ratio be 1:1.
In this example, CH4And O2Mixed gas is incorporated into micro- reaction and set after being sufficiently mixed in 1# reactant mixing apparatus
The micro- reaction channels of 1# in standby, the micro- reaction channels of wherein 1# mixed react scribble partial oxidation reaction of methane on cavity wall
Pt-Ni alloy catalysts, the reaction are carried out at ambient pressure, and mixed reaction gas flow velocity is 3L/min, in micro-reactor apparatus
Residence time is 15ms;Meanwhile CH4And CO2Mixed gas is incorporated into micro- reaction after being sufficiently mixed in 2# reactant mixing apparatus
The micro- reaction channels of 2# in equipment, the micro- reaction channels of wherein 2# mixed react scribble methane carbon dioxide reformation on cavity wall
The active metal Ni catalyst of reaction, the reaction are carried out at ambient pressure, and mixed reaction gas flow velocity is 5L/min, are set in micro- reaction
Residence time in standby is 10ms.Reaction result is as shown in table 1:
Table 1:The reaction result of embodiment 1
Unstripped gas |
Catalyst |
Reaction temperature |
Gas flow rate |
Conversion ratio |
Product yield |
CH4/O2 |
Pt-Ni |
700 oC |
3L/min |
99.6% |
99.7% |
CH4/CO2 |
Ni |
700 oC |
5L/min |
99.2% |
99.5% |
Embodiment 2
With CO and H2Fischer-Tropsch synthesis is carried out for 1# reaction raw materials, the reaction is strong exothermal reaction, wherein CO and H2Between
Ratio is 1:2;With H2And CO2Inverse water gas reaction is carried out for 2# reaction raw materials, the reaction is the endothermic reaction, wherein H2With CO2It
Between ratio be 1:1.
In this example, Fischer-Tropsch synthesis catalyst component is active metal Co, and coal gas catalytic reaction component is Pt against the current,
Before the reaction, two micro- reaction channels in micro-reactor apparatus are first passed through H2450oActivated catalyst 20min under conditions of C.So
Afterwards, it is 350 to control micro-reactor apparatus temperature by temperature automatic adjustment equipmentoC, and(1)By CO and H2Mixed gas is reacted in 1#
The micro- reaction channels of 1# being incorporated into after being sufficiently mixed in thing mixing apparatus in micro-reactor apparatus, reaction pressure 4MPa, mixing are anti-
It is 5L/min to answer gas flow rate,;(2)By CO2And H2Mixed gas is incorporated into micro- after being sufficiently mixed in 2# reactant mixing apparatus
The micro- reaction channels of 2# in consersion unit, reaction pressure 2MPa, mixed reaction gas flow velocity are 5L/min.Wherein F- T synthesis
The CO conversion ratios of reaction are 55.8%, product yield 85.6%;The CO of inverse water gas reaction2Conversion ratio is 99.8%, product yield
For 99.9%.